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Composites: Part A 90 (2016) 22–32

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Composites: Part A
journal homepage: www.elsevier.com/locate/compositesa

A thermo-viscoelastic approach for the characterization and modeling


of the bending behavior of thermoplastic composites
Steffen Ropers a,⇑, Marton Kardos a, Tim A. Osswald b
a
Volkswagen AG, Group Research, Postbox 14990, 38440 Wolfsburg, Germany
b
Polymer Engineering Center, University of Wisconsin-Madison, 1513 University Avenue, Madison, WI 53706, USA

a r t i c l e i n f o a b s t r a c t

Article history: Currently, there is no established and cost-effective method for the bending characterization of continu-
Received 19 January 2016 ous fiber reinforced thermoplastic composites. Isothermal mechanical testing techniques are time and
Received in revised form 6 April 2016 labor-intensive and deliver information only about distinct points of the temperature-dependent
Accepted 18 June 2016
property curves. In this study, Dynamic Mechanical Analysis (DMA) as well as novel rheometer-based
Available online 24 June 2016
bending experiments were performed to assess temperature-dependent and viscoelastic behavior. On
the basis of the experimental results a new method was defined and validated for the efficient
Keywords:
characterization of temperature-dependent elastic bending behavior via DMA. Furthermore a linear
A. Thermoplastic resin
B. Thermomechanical
viscoelastic material model was derived from DMA experiments by means of time–temperature
C. Finite element analysis (FEA) superposition. As the material behavior proved to be of a highly viscoelastic nature, a method was
E. Forming developed to calibrate a material model, the parallel rheological framework, implemented in Abaqus.
Ó 2016 Elsevier Ltd. All rights reserved.

1. Introduction subversions is the most commonly used manufacturing technique


to form continuous fiber-reinforced thermoplastic sheets into com-
The automotive industry is endeavoring to reduce the curb plex geometries. The thermoforming process is governed by the
weights of the vehicles using lower density materials and temperature change of the blank; the organic sheet is first heated
employing lightweight design techniques to meet the stringent above the matrix’ melting temperature, then placed into the mold
safety requirements while reducing emissions. A great number of and formed with relatively low forces. While and after forming, the
non- and semi-structural components have already been replaced sheet rapidly loses heat due to radiation, convection and primarily
by lighter materials, mostly with light metals and unreinforced or heat transfer to the tempered molds. Eventually it consolidates and
fiber-reinforced plastics. Continuous fiber-reinforced plastics exhi- the part is ready for demolding. The changing temperature alters
bit excellent mechanical properties and are capable of substituting the mechanical properties during the forming process. Thus, as
metals in structural applications. The aerospace industry has been pointed out by preceding studies, thermal and mechanical analyses
using these materials for decades, but the automotive segment is need to be fully coupled in the forming simulation of a thermo-
significantly more cost-sensitive [1]. Furthermore, international forming process [2,3].
legislations require new vehicles to be recyclable to a given weight As shown in several studies [2,4–6], the outcome of numerical
percentage. Thermoset resin systems do not possess a re-melting simulations depends significantly on the mechanical properties
capability and are therefore difficult to recycle. Thermoplastic taken into account, hence, properties need to be thoroughly char-
composites solve this problem and simultaneously offer relatively acterized, along with their temperature and other dependencies.
fast cycle times compared to thermoset systems, making them Boisse et al. [4] studied the separated influence of tensile stiff-
very interesting for the automotive industry. Since a trial and error nesses, in-plane shear and out-of-plane bending stiffnesses on
based development is insufficient and costly, virtual prototyping is the forming of a simple geometry and proved the importance of
vital to enable their industrial implementation and cost-effective all three properties. The draping over double curved geometries
development. The thermoforming process along with several requires in-plane shear deformations [2,4] and as the shear stiff-
ness increases with increasing shear angle, wrinkles start to form.
The onset and development of wrinkle formation is a global phe-
⇑ Corresponding author. nomenon that depends on all of the stiffnesses of the material,
E-mail addresses: steffen.ropers@volkswagen.de (S. Ropers), marton.kardos@- however the size and shape of wrinkles is predominantly
volkswagen.de (M. Kardos), tosswald@wisc.edu (T.A. Osswald).

http://dx.doi.org/10.1016/j.compositesa.2016.06.016
1359-835X/Ó 2016 Elsevier Ltd. All rights reserved.
S. Ropers et al. / Composites: Part A 90 (2016) 22–32 23

determined by the out-of-plane bending stiffness [2,4,5,7–9]. Sev- the University of Twente, which is based on the Kawabata Evalua-
eral studies [9,10] have demonstrated the importance of bending tion System and delivers promising results [18]. This latter method
stiffness in the simulation of a forming process. Since wrinkling is capable of investigating the bending stiffness at distinct temper-
is one of the most frequently occurring failures during draping, atures and deformation velocities. The rheometer bending setup
the problem needs to be addressed. was also employed in the framework of this study to acquire the
As pointed out, that material properties need to be understood bending stiffness at predefined temperatures as control values, as
and characterized in order to be able to conduct simulations with discussed in detail in Section 6.
reasonable outcomes. The simulation scale and the material model
determine the involved list of parameters. In a previous study [6]
3. DMA material characterization
the simulation software PAM-FORM, developed by the ESI Group,
was investigated with respect to the influence of different input
Dynamic Mechanical Analysis (DMA) is a mechanical testing
parameters, such as mechanical and thermal material properties.
technique that applies an oscillating deformation to a sample
The simulation is capable of the thermomechanical modeling of
under predefined environmental conditions and analyzes the
the thermoforming process. The Design of Experiments method
material response [19], to study the elastic and viscoelastic proper-
was employed to identify the most influential parameters whose
ties of the material. The method allows for the investigation of a
characterization is worth investing resources into. The Young’s
variety of mechanical and thermal properties and their tempera-
modulus, shear modulus, bending stiffness, specific heat, tool-ply
ture and frequency dependency. DMA instruments are becoming
frictional coefficient and the heat transfer coefficient were proven
even more versatile as state-of-the-art machines offer quasistatic
to be heavily influential on the simulation outcome.
measurement modes to obtain Young’s and other moduli [20],
Internal research at Volkswagen [11] as well as Melo and Rad-
along with creep and relaxation modes [21].
ford [12] have shown that some properties, such as the Young’s
DMA measures the elastic behavior of the material, i.e. stiffness,
modulus in fiber direction, are fiber dominated, meaning that they
and describes it with the storage modulus E0 , which is the in-phase
exhibit only a small temperature dependency in the investigated
component of the reaction to the applied sinusoidal deformation.
temperature range. It is sufficient to only characterize these prop-
The loss modulus E00 is the out-of-phase component describing
erties at distinct temperatures with conventional mechanical test-
the material’s ability to dissipate energy into heat, and the ratio
ing methods. Other properties, however, are matrix dominated and
of the loss to the storage modulus is the so-called tand, i.e. damping
therefore heavily temperature-dependent. Such properties are
[19].
transverse Young’s modulus, shear modulus and out-of-plane
Researchers use DMA to characterize polymers usually below
bending stiffness. The characterization of the shear modulus and
their melting temperature. Melo et al. [12] investigated the vis-
the bending stiffness is particularly challenging, especially due to
coelastic properties of unidirectional carbon fiber reinforced PEEK
their additional deflection and shear rate dependencies. There is
tapes, but only at a temperature range below the matrix materials
no established method for the efficient characterization of these
glass transition temperature (T g ). Other studies [22,23] employed
properties [8].
DMA to examine the temperature-dependent elastic moduli of
epoxies and to compare them to conventional mechanical testing
data. They found discrepancies between the actual values but good
2. Methods for bending characterization
correlation between their temperature dependencies. Margossian
et al. [5] presented a DMA-based characterization method for the
The bending stiffness of continuous materials is classically
bending behavior of unidirectional composite tapes. The study
derived from their in-plane properties [13]. However, the investi-
was conducted under the assumption that experimental forming
gations of Yu et al. [14] have shown that the calculated bending
methods are mostly modeled as isothermal processes. Thus, the
stiffness is unrealistically high compared to the experimentally
study focuses on characterizing the material’s bending behavior
obtained value of a fiber-reinforcement. This can be attributed to
at distinct temperatures, instead of doing temperature sweeps over
sliding mechanisms between the yarns and individual fibers of
a broader range. Such a characterization method yields insufficient
the reinforcement, which assign a specific bending behavior to
data for thermomechanical simulations. A great number of isother-
the reinforcement that is independent of the tensile and shear
mal measurements would be required to characterize the temper-
properties and, therefore, cannot be deduced from the calculated
ature range in question, which brings us back to the inefficiency of
values [9,15]. Modern simulation software and material models
common mechanical testing techniques.
are aware of that and require an independent bending stiffness
The method proposed in this study enables the fast and efficient
to be defined for main fiber directions. Thus, bending characteriza-
characterization of both temperature and frequency dependencies
tion is a vital requirement for forming simulations.
of the bending stiffness, however, it does not deliver the actual
Only few studies have been carried out to date on the bending
bending stiffness values. The technique requires the bending stiff-
characterization of continuous fiber reinforced thermoplastic com-
ness to be determined at least at one temperature within the inves-
posites in their molten state [5,9,10,16]. Conventional bending test
tigated range.
methods are inapplicable to materials with low bending stiffness
such as dry reinforcement fabrics and molten state thermoplastic
prepregs. The testing techniques developed by the textile industry 4. Materials and instruments
were used as the basis for the development of techniques applica-
ble to such materials. Most bending characterization techniques All experiments were performed on two materials; both
are based on the cantilever or the Kawabata tests, which both orig- representing the most commonly used thermoplastic prepreg
inate from the textile industry. Several studies employed a modi- types. The first investigated material is a woven textile reinforced
fied version of the cantilever test to characterize the bending thermoplastic prepreg (TPP) material, Tepex 102 dynalite-RG600
behavior, such as those conducted by Boisse [4] or Peirce [17]. Mar- (x)/47% supplied by Bond-Laminates. The prepreg consist of a 2/2
gossian [5] presented an extensive review of the existing test twill glass fiber weave impregnated with a polyamide 6 (PA6)
methods for bending characterization, explaining various versions matrix. Main properties of the material are listed in the material
of the cantilever test, the Kawabata test and the V-bending test. data sheet provided by the manufacturer [24] and listed in Table 1.
The study also mentions the modified rheometer developed by The second material is a continuous unidirectional carbon fiber
24 S. Ropers et al. / Composites: Part A 90 (2016) 22–32

Table 1 ple while continuously sweeping through a temperature range. The


Main material properties. rheometer bending experiments were conducted in a standard
Trade name Tepex dynalite Ultratape rheometer instrument employing a custom built bending fixture
102-RG600(x)/47% B3EC12 UD02 that allows for the measurement of the material’s response to sub-
Matrix PA6 PA6 stantial bending deformation under isothermal conditions.
Fibers Glass Carbon
Reinforcement type Twill weave 2/2 UD
Fiber volume (%) 47 50 5.1. DMA experiments
Density (g/cm3) 1.8 1.46
Thickness (mm) 0.5 0.16
Three of the available test methods are applicable to the charac-
terization of out-of-plane bending: three-point bending, single-
cantilever and dual-cantilever. Most previous studies employing
reinforced thermoplastic composite tape with a polyamide 6 DMA used the three-point bending deformation method
matrix, called Ultratape B3EC12 UD01 black supplied by BASF. [5,12,22], motivated by the elimination of clamping effects inher-
Basic material properties can be found in its material data sheet ent in the cantilever clamping system. However, when conducting
and are also listed in Table 1. dynamic measurements, three-point-bending is not applicable to
Since the resulting storage modulus values are only used for the investigated materials above melting temperature. The sample
comparison and not to determine the actual bending stiffness, is not clamped by the three-point-bending fixture, only supported.
the specimens were not conditioned to control their moisture con- Therefore, the sample will not follow the oscillating stamp once
tent. However, prior to testing each specimen was stored under the the sample loses most of its elastic bending properties due to being
same conditions to ensure that the results are comparable. heated above melting temperature, creating a gap between sample
The DMA instrument used to conduct the experiments was a and stamp and corrupting the test. Then again, cantilever clamping
Netzsch DMA 242 Artemis E. The dynamic deformation amplitude systems introduce an additional shearing component to the distor-
of the machine is limited to 240 lm, and the maximum dynamic tion [5,19,12,22]. This issue can be overcome by introducing shear
force is 12 N. Several deformation methods and corresponding correction to the calculation. However, this study uses DMA results
sample holders are available for the device. One of the basic out- for comparison, thus introducing a shear correction to both sides of
puts of the analysis is the storage modulus, which is conceptually the equation would have been inexpedient. The single cantilever
similar to other moduli. Depending on the deformation method deformation method would be applicable to the material, but the
used, the storage modulus may represent tensile, shear or flexural dual cantilever sample holder allows for a more robust clamping
modulus [19,22]. The other two basic outputs are loss modulus and of the material. Since the two methods are principally identical,
damping. only the dual cantilever system, see Fig. 2 was taken into consider-
Mechanical bending experiments were conducted on a modi- ation in the scope of this work. All tests conducted within this
fied rheometer to characterize the bending behavior of both inves- study were dynamic temperature sweeps applying an oscillating
tigated materials. The device was developed at the University of force at multiple frequencies, carried out with the dual-cantilever
Twente by Sachs [18] based on the Kawabata Evaluation System deformation system.
(KES). The rheometer is equipped with a thermal chamber, which Margossian [5] reported to have encountered difficulties with
enables a precise temperature control throughout the experiment. the dual-cantilever sample holder above and around melting tem-
A special fixture was designed for the rheometer; see Fig. 1. As the perature, as the fixture appeared to be instable. Within the scope of
rotating part of the fixture moves on a circular path, the free arc this work no instability issues were encountered with the sample
length changes with the angle a. The specimen is not clamped holder system while conducting the experiments.
but resting loosely in the fixture on support pins to avoid tensional The specimens were clamped in the fixtures using 30 cN m of
or compressional strains in the specimen. The device allows for torque to tighten the bolts. The bolts were not retightened during
testing at various temperatures while different rotational velocities the experiments. The environmental chamber was heated to the
can be applied to deform the specimen in order to identify strain starting temperature with a heating rate of 10 K min1. To ensure
rate dependencies of the bending behavior. Sachs used this device a homogeneous sample temperature, a 20 min balancing time
to test a thermoplastic UD tape with different thicknesses (number
of plies) and at different rotational velocities and temperatures.

5. Implementation

Standard DMA cantilever-bending tests were conducted, where


minuscule sinusoidal forces, or deflections, are applied to the sam-

Fig. 1. Experimental set-up in rheometer for bending experiments [18]. Fig. 2. Dynamic mechanical analysis: dual cantilever fixture.
S. Ropers et al. / Composites: Part A 90 (2016) 22–32 25

was used. The heating rate was set to 1.5 K min1 during the exper- Table 2
iments. The environmental chamber was continuously flushed Investigated materials and parameters in rheometer bending tests.

with nitrogen in order to avoid polymer oxidation at elevated Materials Temperatures (°C) Rotational velocities (rpm)
temperatures. Tepex 60/150/210/220/ 0.1/1/10
Temperature-sweeps were conducted from 150 °C to 260 °C. Ultratape 210+/220+/260
150 °C was chosen as the lower limit of the investigated tempera-
ture range, as it is a favorable mold temperature for thermoform-
ing PA6 materials. It is very unlikely that the blank temperature tional velocities will further be referred to as 0.1 rpm (rotations
would drop below 150 °C during the swift forming process. The per minute), 1 rpm and 10 rpm.
upper limit was chosen to be 260 °C, because this is the upper limit Crystal melting is an endothermic transition, while crystalliza-
of the processing temperature range defined by the prepreg man- tion is exothermic. When cooling the environmental chamber from
ufacturer. At higher temperatures the matrix material is prone to above the melting temperature, the sample will consolidate and
temperature degradation; furthermore, the mechanical properties crystallize, while giving off heat. This keeps the sample warm
are not changing significantly once complete melting has occurred. and shifts the apparent melting temperature to a lower value.
Six frequencies from 0.1 Hz to 10 Hz were investigated: 0.1, 0.5, Therefore, bending tests around melting temperature T m were per-
1, 2, 5 and 10 Hz. The maximum amplitude of the employed DMA formed both while heating up and while cooling down after over-
instrument is 0.24 mm. It takes a quarter of the cycle time for the heating. As expected, the experiments conducted while cooling the
stamp to get from the initial position to the maximum amplitude. sample from a temperature > T m delivered significantly lower
At a 10 Hz frequency this means that the sample is flexed 0.24 mm mechanical properties, as the material still exhibited molten state
in 0.025 s, which roughly corresponds to a punch velocity of behavior. Thus, tests were performed at 60 °C, 150 °C, 210 °C,
10 mm s1. The actual strain rate of the blank during draping is 220 °C and 260 °C without overheating, furthermore, at 210 °C
geometry dependent and non-uniform, but this has not been and 220 °C with overheating to 255 °C and cooling back to 210 °C
accounted for in this study. This is a necessary simplification in and 220 °C (indicated with ‘‘+” henceforth and in Table 2), respec-
order to limit the complexity of the model. tively, to identify the shift in behavior due to crystallization and
Five experiments were made for both directions and both mate- crystal melting. After reaching the experimental temperature, a
rial types. According to the material data sheet, there is a small dif- two minute balancing time was employed to ensure a homoge-
ference between mechanical properties in weft and warp neous temperature field in the sample during the test. The mea-
directions. This can be attributed to the prepreg manufacturing sured temperature, however, might differ from the actual sample
technique that pulls the weft rovings out of alignment by slightly temperature during the measurements, due to the following
bending them. This difference was investigated by conducting reasons:
DMA measurements on samples cut in both directions. The result-
ing difference was deemed to be negligible, henceforth only warp  Temperature sensor was not inside/not in contact with the
direction results were taken into account. sample.
The result of DMA measurements are the complex modulus E  Heating rate was relatively high.
with its real and imaginary parts E0 and E00 which denote the stor-  Balancing time might not be sufficient to reach homogeneous
age and loss modulus respectively. temperature field.

E ¼ E0 þ ıE00 ð1Þ
6. Experimental results
0
The storage modulus E describes the material’s ability to store
the deformation energy while the loss modulus E00 describes the In the following section the results of DMA bending and
ratio of the deformation energy which is transformed into heat rheometer experiments will be presented.
by dissipation. Their ratio is usually referred to as tan d or damping.
6.1. DMA experiments
E00
tan d ¼ ð2Þ
E0 Twenty DMA measurements were made; five for both direc-
tions for both materials. As previously discussed, only warp direc-
tion results of the fabric and longitudinal results of the tape are
5.2. Rheometer bending experiments
considered in the analysis. The storage modulus values of the five
identical measurements were averaged for every frequency tested.
The rheometer bending setup was used in the scope of this
Three frequencies are being further investigated: 0.1, 1 and 10 Hz.
work to investigate the bending behavior of single plies of Tepex
These roughly correspond to the angular velocities used in the
and Ultratape material. Additionally to the experimental procedure
rheometer measurements. Fig. 4 shows the average storage and
performed by Sachs, relaxation was also investigated. After bend-
loss modulus as well as damping curves for these three frequen-
ing the specimen from 0° to 70° the bending angle was held at
cies. The damping exhibits more distinctive frequency dependence
70° for another 120 s, while measuring the reaction moment.
owing to the viscous behavior of the molten thermoplastic.
Fig. 3 gives an overview of the test procedure:
These averaged storage modulus values were then converted
The tested parameters and their settings are listed in Table 2.
Three bending rates were tested at five temperatures. The rota- into proportionality P i factors by dividing every value E0i with the
base value E0base , i.e. the storage modulus corresponding to the low-
est investigated temperature:

E0 ðT i Þ
PðT i Þ ¼ : ð3Þ
E0 ðT base Þ
Thus, an array of proportionality factors starts with a value of
one (corresponding to the base temperature) and gradually
Fig. 3. Rheometer bending test procedure. decreases to a value less than one, which shows how much smaller
26 S. Ropers et al. / Composites: Part A 90 (2016) 22–32

pointed out by Deng [22], needs to be assessed thoroughly involv-


ing a wide variety of materials and deformation methods, which
will be the scope of future studies.
The rheometer bending results yield the bending stiffness at
five investigated temperatures. Two temperatures, i.e. 210 °C and
220 °C were investigated both while heating up and while cooling
down from a temperature > T m , because these are located in the
transitional region of melting. Due to reasons discussed in Sec-
tion 5.2, discrepancies between the actual sample temperature
and the measured temperature might occur. Furthermore, the
melting temperature differs from the consolidation temperature,
as the results obtained at 210 °C and 220 °C with overheating, have
shown. Therefore, the bending stiffness values acquired at 210 °C
and 220 °C with overheating were shifted to 20 K higher tempera-
tures, to account for this discrepancy. The triangles in Fig. 5 repre-
Fig. 4. Resulting storage modulus, loss modulus and damping for Tepex material at sent the original bending stiffness values calculated from the
0.1, 1 and 10 Hz. rheometer bending results, while the squares show their positions
after the shift.
This shift by 20 K of the overheated measurement points is nec-
the storage modulus is at the highest temperature investigated. essary due to the aforementioned uncertainties regarding the exact
Such a set of proportionality factors describes the storage modulus’ specimen temperature as well as the definite difference regarding
temperature dependency at a given frequency. Multiplying the the state of the thermoplastic matrix depending on whether the
proportionality factors with the bending stiffness measured at samples were preheated to 255 °C or not. Plotting the DMA storage
the base temperature delivers a set of predicted bending stiffnesses modulus curve at both heating up and cooling down shows an
for the entire temperature range. These predicted values were approximate 20 K discrepancy between the melting and the crys-
compared with the bending stiffness values calculated from the tallization temperature, as shown in Fig. 6. The same effect can
TPRC rheometer measurement results, to validate the proposed be observed on differential scanning calorimetry diagrams as the
characterization method. Fig. 5 plots the six bending stiffness val- offset between the endo-and exothermic peaks of melting and
ues derived from the rheometer bending results, along with the crystallization, respectively. The effect is due to thermal inertia,
predicted values delivered by the proposed DMA-based method. since the endothermic physical reaction of crystal melting is taking
Other studies [12,22,23] employing dynamic mechanical analy- up extra thermal energy while the exothermic crystallization is
sis for material characterization found that the temperature and heating the material from the inside [3]. This discrepancy was
frequency dependency of viscoelastic material properties can be determined separately for both Tepex and Ultratape materials
adequately studied with DMA. However, DMA derived storage based on the DMA storage modulus curves, as seen in Fig. 6, and
moduli are known to show considerable discrepancies to mechan- was found to be approx. 20 K for both materials. This is the
ical testing moduli regarding their absolute values. Hobbibrunken expected result since both materials consist of the same PA6
[23] calibrated the DMA derived moduli curves by shifting them matrix and the bending behavior was presumed to be matrix dom-
to a lower temperature to fit the mechanical testing results. Deng inated. Furthermore, the results in the transitional region are
[22] compared the DMA storage modulus to the Young’s modulus highly dependent on factors such as heating rate and balancing
measured by mechanical testing at the same temperature and time. Therefore, the results do not correlate perfectly with the pre-
shifted all storage modulus values with the difference, producing dicted curve, although exhibiting the same trend regarding tem-
a shifted moduli curve. This latter shift method was applied to perature dependency, see Fig. 5. The accurate measurement of
the storage modulus of the Tepex material to demonstrate its inap- mechanical properties in this region requires further investigation.
plicability to thermoplastic materials investigated over a broad Nevertheless, the molten state stiffness at 260 °C was successfully
temperature range involving transitions, as shown by the blue line predicted for both materials with outstanding accuracy.
in Fig. 5(a). The proposed proportionality method overcomes these Fig. 5 reveals that the bending stiffness curve derived from the
issues for both material types, as proven by the comparison plotted DMA storage moduli shows good correlation with the data
in Fig. 5. However, the validity of such manipulation, as also acquired from the rheometer bending measurements, especially

Fig. 5. Comparison of predicted and experimental bending stiffness.


S. Ropers et al. / Composites: Part A 90 (2016) 22–32 27

depicted in Fig. 8. This is due to the moment of inertia of the instru-


ment and the sample holder.
Time, bending angle and bending moment were documented
during the measurements. Three measurements were carried out
for every setting, the results of these have been averaged. The over-
all reproducibility was excellent, due to the outstanding velocity
control of the rheometer. The experimental results have proven
the materials’ strong temperature dependency, as exemplary
shown for the UD Ultratape material in Fig. 9 (a) and (b), displaying
the bending behavior below and above melting temperature,
respectively. The experiments also revealed the significant rate
dependency of the bending behavior for both investigated materials
above melting temperature. The material response is elastic at 60 °C
and 150 °C, i.e., beneath T m , and is therefore barely rate dependent,
as illustrated by Fig. 9 (c). The response at 210 °C and 220 °C with-
out overheating was also mostly elastic but has been disturbed by
Fig. 6. Difference between melting temperature and recrystallization temperature the buckling of the material instead of a homogeneously distributed
of Tepex. bending. At 210 °C and 220 °C with overheating and 260 °C the
response showed a typical viscoelastic material behavior exhibiting
strong rate dependency and significant relaxation after deforma-
tion onto the same level of bending moment independent of the
velocity, see exemplary Fig. 9 (d). The fabric Tepex material showed
very similar behavior over the whole tested temperature and rota-
tional velocity ranges. Fig. 10 is an exemplary output for varying
temperature and 10 rpm velocity.
The bending angles have been used to calculate the correspond-
ing curvature j of the sample by:
a
j¼ ; ð4Þ
lb
where a is the bending angle in radiant and lb is the bending length
in mm. The initial bending length changes with the bending angle,
due to geometrical relations. The bending length was calculated
from the bending angle:
a
lb ¼ aR tan1 ; ð5Þ
2
where a is again the bending angle in radiant and R is the bending
Fig. 7. Proportionality factors for both materials, Tepex and Ultratape, versus radius in mm. The initial bending length (a ¼ 0) was 15 mm, since
temperature.
the rheometer’s bending radius is 7.5 mm.
The bending stiffness B was calculated from the bending
regarding the prediction of the molten state stiffness. Plotting the
moment M, curvature j and the area moment of inertia I:
proportionality factors for both the Tepex und Ultratape materials,
see Fig. 7, also proves that the change of the bending behavior over M
B¼ : ð6Þ
temperature is matrix dominated. Thus, the proportionality factors jI
exhibit a nearly identical course in the investigated temperature
The calculated bending stiffness of both materials shows an ini-
range, even though the bending stiffness of the Ultratape material
tial unsettled section until a curvature of approximately 0.02–
is an order of magnitude higher than that of the Tepex material.
0.03 mm1. This phenomenon is present irrespective of tempera-
Nonetheless, proportionality factors for bending stiffness predic-
ture and bending velocity. After this initial unsteady region, the
tion were calculated separately for Ultratape and Tepex.
bending stiffness is linearly increasing below melting temperature
Further research is due on a wider range of materials to prop-
and slightly decreasing above T m . At 220 °C without overheating
erly validate the method, but this first validation attempt proves
the material experienced buckling, hence the distinct shape of
the method to be very promising. The proposed method has the
the curve. Therefore, approximately the first half of the bending
potential to significantly decrease the time and effort required
movement was neglected in the analysis. The bending stiffness val-
for the characterization of temperature-dependent mechanical
ues were thus averaged over the second half of the bending range
properties. Therefore, it will speed up the virtual prototyping pro-
between 0.04 and 0.08 mm1 curvatures (a  35 . . . 60 ). This
cess while delivering higher quality simulation input data. It is
range describes the long-term bending behavior.
important to note that the method was applied to linear-elastic
Both DMA and rheometer experiments revealed highly vis-
bending stiffnesses. PAM-FORM among other commercial tools
coelastic material behavior in the molten state. The rheometer
uses an elastic approach for the bending stiffness, thus this method
bending results delivered bending moments which largely
is very valuable for such simulation tools.
depended on the deformation speeds. Higher deformation speeds
resulted in up to doubled bending moments with respect to lower
6.2. Rheometer bending experiments deformation speeds. Liang et al. [9] deemed the influence of the
bending stiffness on the wrinkling behavior in forming simulation
The rheometer exhibited a perfect velocity control even at the results as small, as only variations of one magnitude resulted in
highest investigated speed. The torque response, however, shows visible differences in the used research-state draping simulation
a strong fluctuation in the initial region of the measurements, as tool. However, in a quantitative sensitivity study of the simulation
28 S. Ropers et al. / Composites: Part A 90 (2016) 22–32

Fig. 8. Fluctuations in moment signals due to inertia of instrument and sample holder.

Fig. 9. Influence of temperature and rotational velocity on bending behavior of the


Ultratape material. Fig. 10. Influence of temperature on bending behavior of the Tepex material.
S. Ropers et al. / Composites: Part A 90 (2016) 22–32 29

perature. Ferry [25] described that an increase in temperature is


equal to a contraction of relaxation times with respect to the mate-
rial response to a load. The principle of time–temperature superpo-
sition (TTS) is based on this observation. As DMA machines are
usually equipped with a thermal chamber (cooled with nitrogen),
testing over a wide temperature range is possible while the neces-
sary time scale cannot be realized or would be inefficient. The
resulting dynamic moduli for each of the temperature points along
the temperature range are shifted by shift factors aT along the time
axis so that a continuous curve results, see following Fig. 12. This
curve is called master curve and defines the viscoelastic material
(a) Bending stiffness (b) Bending stiffness behavior at an arbitrary reference temperature. Corresponding
base value multiplied by 2 curves for the other temperature points are retrieved by a horizon-
tal shift of the master curve by the given temperature’s aT .
Fig. 11. Sensitivity analysis on the bending stiffness: bending stiffness at base value The shift factors are usually given by the Williams-Landel-Ferry
(a) and bending stiffness multiplied by 2 (b). (WLF) equation [25]

tool PAM-FORM [6], the influence of the bending stiffness even on C 1 ðT  T 0 Þ


log aT ¼  ; ð7Þ
the shear angle of the examined fabric material was in the magni- C 2 þ ðT  T 0 Þ
tude of the shear modulus. In order to estimate the influence of the or the Arrhenius equation. T 0 represents the chosen reference tem-
bending stiffness on the forming result, two simulations were run perature and C 1 and C 2 are material specific parameters to fit the
in PAM-FORM on a half-dome geometry with only a difference in equation to the determined shift factors. The viscoelastic behavior
bending stiffness of a factor of 2. The results are depicted in given by the master curve can be represented by a series of Prony
Fig. 11. Doubling the bending stiffness results in a clearly different terms, which represent a series of Maxwell elements and a spring:
forming result.
Therefore, the bending stiffness is one parameter which needs X
n
EðtÞ ¼ E1 þ Ei eðt=si Þ : ð8Þ
to be thoroughly characterized in order to realistically predict i¼1
shearing and wrinkling of thermoplastic prepregs.
Thus, in order to further improve the predictability of draping E1 defines the long-term behavior, while each Ei has a corre-
simulations, viscoelastic material models need to be implemented, sponding relaxation time si .
validated and fitted to corresponding experimental results. Sachs The principle of time–temperature superposition and the sub-
[18] developed a viscoelastic bending model for thermoplastic sequent description of the material behavior with Prony terms
UD tapes based on their composition of thermoplastic matrix and and a shift function is usually applied for the transition from glassy
fiber layers. Yet the parameters had to be adapted to different con- to rubbery behavior at the glass transition temperature T g for non-
ditions as temperature or rotational velocity. Thus, in the following continuous fiber reinforced polymers. As the measured continuous
section an attempt is made to find a general model for the material fiber-reinforced polymers are still almost entirely elastic above T g
behavior of thermoplastic prepregs under bending. and the shape of the transition of the storage modulus at T g and T m
is similar, it was assumed that time–temperature superposition is
applicable for the transition to the molten state as well. Thus, for
7. Viscoelastic material models for bending behavior the performed DMA measurements a Prony series with 20 ele-
ments (n ¼ 20) and a WLF representation of the shift factors were
7.1. Linear viscoelastic model using Prony series derived for the Tepex fabric and the Ultratape UD material. These
were used to define a temperature-dependent linear viscoelastic
The DMA experiments reveal a clearly viscoelastic bending material model in Abaqus. The WLF function has a change of sign
behavior of thermoplastic prepregs. Polymers show a high depen- at the temperature T sign ¼ T 0  C 2 . Abaqus uses for any tempera-
dency of their mechanical properties on time/frequency and tem- ture lower than T sign the same shift factor aT as for T sign .

Fig. 12. Time–temperature superposition of the storage modulus.


30 S. Ropers et al. / Composites: Part A 90 (2016) 22–32

Fig. 13. Simulated and experimental maximum bending moments at speed 10 rpm versus temperature.

The material model derived from the DMA measurements was


used to simulate the bending experiments performed with the
rheometer. As the material model is linear viscoelastic but the
experimental curves are highly non-linear only the maximum
bending moments at 70° deflection were compared. The simula-
tions were run at constant temperatures of 150 °C, 200 °C,
210 °C, 220 °C, 240 °C and 260 °C. The resulting maximum bending
moments, along with the bending moments derived from the
rheometer measurements are depicted in Fig. 13. The bending
moments obtained from the rheomter bending measurements
done at 210 °C and 220 °C with overheating were shifted to 20 K Fig. 14. Schematic of parallel rheological framework with one hyperelastic element
”0” and three viscoelastic elements 1–3.
higher temperatures to 230 °C and 240 °C, (similarly to those
shown in Fig. 5) for the same reasons discussed in Section 6.1.  n  1
For the Ultratape material the correlation between the simula- _ cr ¼ Aq
~ ½ðm þ 1Þcr m mþ1 ; ð9Þ
tion results and the experimental moment values is excellent over
where _ cr is the creep strain rate cr is the creep strain, q
~ is the devi-
the whole investigated temperature range, especially at 210 °C and
220 °C, as shown in Fig. 13(b). (Notice that the y-axis of the dia- atoric Kirchhoff stress A; m and n are parameters unique to the
material. The elastic elements are all specified by hyperelastic
grams have a logarithmic scale). The largest difference between
the results can be seen at 150 °C, since the WLF model was fit for material models which are isotropic and nonlinear. The strain
energy stored in the material per reference volume, the so-called
the range of 190 °C to 260 °C.
For the Tepex material all predicted maximum bending strain energy potential, describes the behavior of hyperelastic mate-
rials as a function of the strain.
moments are lower than the experimental results, although the
temperature dependency shows a very similar trend. This could For the description of the material behavior under bending of
the thermoplastic prepregs, a reduced polynomial form of the
be due to the fact that the Prony series are derived from minuscule
strains from the DMA tests while the material exhibits a highly strain energy potential was used, which has the general form
non-linear bending behavior at high strains. The woven reinforce- Xn
 i Xn
1  el 2i
ment structure of Tepex results in a more complex bending behav- U¼ C i0 I1  3 þ J 1 ; ð10Þ
i¼1 i¼1
Di
ior due to the inherent undulation of the fiber rovings, while the
simple structure of the unidirectional reinforcement allows for a where n was set to 3 which then corresponds to the Yeoh model
behavior that is easier to predict. Nevertheless, the onset and rate [28]. U is the strain energy per unit of reference volume, C i0 and
of stiffening with decreasing temperature is quite similar in exper- Di are material parameters and I1 is the first deviatoric strain invari-
iments and simulation. This comparison again justifies the trans- ant. For further details the reader is referred to the Abaqus manual
ferability of the temperature dependency of the elastic moduli [29].
derived from the DMA onto the bending stiffness. The material parameters of both the hyperelastic and the vis-
cous elements were fitted to the results of the rheometer bending
7.2. Non-linear viscoelastic model using parallel rheological experiments. Therefore, the experimental bending angles and
framework bending moments were translated into strains and stresses. As
for high deformations there is no analytical correlation between
The parallel rheological framework (PRF) [26] in Abaqus enables curvatures or bending moments and strains or stresses, respec-
the definition of a customized viscoelastic material. Therefore, the tively. A tool was developed which creates the correlation itera-
user can define any number of parallel viscoelastic elements to tively. An optimization algorithm was used to fit the model
model polymers that exhibit non-transient deformations and non- parameters to the corresponding strain stress curves of the differ-
linear viscous behavior under large deformations. Fig. 14 exhibits ent rotational speeds. Thus, each subsequent iteration lets the
an exemplary framework with four elements, which was used in this material model and thus the simulation results approach the
work. For every element the share of the overall material response is experimental results. The rheometer bending experiments were
P
defined by a stiffness ratio S. The sum of the stiffness ratios S is modeled with solid elements using two elements over the thick-
P
equal to or smaller than 1. If S equals unity no pure elastic element ness, as the parallel rheological framework is limited to solid ele-
P
”0” is added. In case the sum of the ratios S is smaller than 1, an ments. Friction was neglected.
P
elastic element ”0” with the stiffness ratio 1  S is added. First, a simulation for each investigated bending speed (0.1 rpm,
In the scope of this work, for the viscous elements a Power-law 1 rpm, 10 rpm) was run with the initial material parameters. The
strain hardening model was used [27]: simulation outputs were analyzed and stress, strain, reaction
S. Ropers et al. / Composites: Part A 90 (2016) 22–32 31

moment and bending angle results were extracted for every incre-
ment. Thus, the correlation between logarithmic strain and bend-
ing angle as well as stress and reaction moment was established,
separately for each bending velocity. On the basis of this correla-
tion, strains and the ratios of stresses to reaction moments were
linearly interpolated corresponding to the bending angles of the
rheometer measurements. The resulting ratios of stress to reaction
moment were multiplied with the reaction moments from the
rheometer measurements, thus delivering the stress values corre-
sponding to the strains. The resulting stress–strain data was used
to calibrate the material model employed in the simulations to cor-
respond to the experimental results. The calibration was done via
an automated iteration process. The obtained material model has
then been implemented in the subsequent array of simulations.
This process was repeated until the simulation results showed an
acceptable correlation to the experiments. Such a process is shown
in Fig. 15. The same material model parameters were used for all
Fig. 16. Experimental and simulated bending moment of Tepex at 220 °C and 1 rpm
rotational velocities. The corresponding result for the 1 rpm speed rotational velocity.
is depicted in Fig. 16.
Figs. 15 and 16 clarify, that a non-linear viscoelastic material
model is capable of representing the actual material bending
behavior of thermoplastic prepregs. The results delivered by the
employed parallel rheological framework not only fit the experi-
mental results during the deformation of the specimen but also
accurately represent the relaxation behavior. The developed
method of coupling an iterative process with a calibration algo-
rithm allows for an efficient and robust determination of material
model parameters.

7.3. Combination of time–temperature superposition and non-linear


viscoelastic model

The method for determining the parameters of the non-linear


viscoelastic parallel rheological framework mentioned in the previ-
ous section was also successfully applied to the rheometer bending
results at a different temperature point, 210 °C. As the principle of
time–temperature superposition was deemed to be applicable for
Fig. 17. Experimental and simulated bending moment of Tepex at 210 °C and
the change in behavior over the temperature for the linear vis- 10 rpm rotational velocity.
coelastic material with a Prony series it was applied here as well.
The parameters for the parallel rheological framework for 220 °C
were used and each viscoelastic element was given a temperature
time shift in the form of the WLF equation and the corresponding
parameters C 1 and C 2 . The reference temperature T 0 was corre-
spondingly set to 220 °C. Fig. 17 exhibits the results at the
10 rpm velocity for a separate fit of the parallel rheological frame-
work parameters for 210 °C and the results of the shifted 220 °C

Fig. 18. Experimental and simulated bending moment of Tepex at 210 °C and 1 rpm
rotational velocity.

parameters. Both results are in correlation with the experimental


results. The shifted material model was also applied to the 1 rpm
velocity, see Fig. 18. As a temperature time shift is capable of
Fig. 15. Depiction of iterative process, experimental and simulated bending representing the material behavior at a temperature different to
moment of Tepex at 220 °C and 10 rpm rotational velocity. the reference temperature at 1 rpm and 10 rpm velocity, it is
32 S. Ropers et al. / Composites: Part A 90 (2016) 22–32

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